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Journal Article

Temperature effects on singlet fission dynamics mediated by a conical intersection

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Sun, K., Xu, Q., Chen, L., Gelin, M. F., & Zhao, Y. (2020). Temperature effects on singlet fission dynamics mediated by a conical intersection. The Journal of Chemical Physics, 153(19): 194106. doi:10.1063/5.0031435.

Cite as: http://hdl.handle.net/21.11116/0000-0007-F5E7-0
Finite-temperature dynamics of singlet fission in crystalline rubrene is investigated by utilizing the Dirac-Frenkel time-dependent variational method in combination with multiple Davydov D-2 trial states. To probe temperature effects on the singlet fission process mediated by a conical intersection, the variational method is extended to include number state propagation with thermally averaged Boltzmann distribution as initialization. This allows us to simulate two-dimensional electronic spectroscopic signals of two-mode and three-mode models of crystalline rubrene in the temperature range from 0 K to 300 K. It is demonstrated that an elevated temperature facilitates excitonic population transfer and accelerates the singlet fission process. In addition, increasing temperature leads to dramatic changes in two-dimensional spectra, thanks to temperature-dependent electronic dephasing and to an increased number of system eigenstates amenable to spectroscopic probing.